• Energy Research

AbstractAtmospheric aerosols and their effect on clouds are thought to be important for anthropogenic radiative forcing of the climate, yet remain poorly understood1. Globally, around half of cloud condensation nuclei originate from nucleation of atmospheric vapours2. It is thought that sulfuric acid is essential to initiate most particle formation in the atmosphere3,4, and that ions have a relatively minor role5. Some laboratory studies, however, have reported organic particle formation without the intentional addition of sulfuric acid, although contamination could not be excluded6,7. Here we present evidence for the formation of aerosol particles from highly oxidized biogenic vapours in the absence of sulfuric acid in a large chamber under atmospheric conditions. The highly oxygenated molecules (HOMs) are produced by ozonolysis of α-pinene. We find that ions from Galactic cosmic rays increase the nucleation rate by one to two orders of magnitude compared with neutral nucleation. Our experimental findings are supported by quantum chemical calculations of the cluster binding energies of representative HOMs. Ion-induced nucleation of pure organic particles constitutes a potentially widespread source of aerosol particles in terrestrial environments with low sulfuric acid pollution.

Abstract. Secondary aerosol is a major component of PM2.5, yet its formation mechanism in the ambient atmosphere is still an open question. Based on field measurements in downtown Beijing, we show that the photolysis of nitrous acid (HONO) could promote the formation of organic and nitrate aerosol in wintertime Beijing as evidenced by the growth of the mass concentration of organic and nitrate aerosols linearly increasing as a function of consumed HONO from early morning to noon. The increased nitrate also lead to the formation of particulate matter ammonium by enhancing the neutralization of nitric acid by ammonia. We further illustrate that over 50 % of the ambient HONO during pollution events in wintertime Beijing might be related to traffic-related emission including direct emission and formation via the reaction between OH and vehicle-emitted NO. Overall, our results highlight that the traffic-related HONO plays an important role in the oxidative capacity and in turn, contribute to the haze formation in winter Beijing. Mitigation of HONO and NOx emission from the vehicles might be an effective way to reduce secondary aerosol mass formation and severe haze events in wintertime Beijing.